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对源自金属有机框架的锰钴氧化物用于甲苯完全氧化的高性能的见解。

Insights into the high performance of Mn-Co oxides derived from metal-organic frameworks for total toluene oxidation.

作者信息

Luo Yongjin, Zheng Yingbin, Zuo Jiachang, Feng Xiaoshan, Wang Xiuyun, Zhang Tianhua, Zhang Kai, Jiang Lilong

机构信息

Fujian Key Laboratory of Pollution Control & Resource Reuse, Fujian Normal University, Fuzhou 350007, PR China.

National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, PR China.

出版信息

J Hazard Mater. 2018 May 5;349:119-127. doi: 10.1016/j.jhazmat.2018.01.053. Epub 2018 Jan 31.

Abstract

Mn-Co mixed metal oxide is considered as efficient catalyst for the total oxidation of volatile organic compounds. In this study, nanocube-like metal-organic frameworks (Mn[Co(CN)]·nHO) are adopted as the precursor to generate Mn-Co oxides with different Mn/Co molar ratios, which affect little on phase structure and textural properties. The obtained MOF-Mn1Co1 with uniform metal dispersion is rich in high valence of surface Mn and Co species, leading to high low-temperature catalytic activity of total toluene oxidation. The results of toluene-TPD followed by TPO and toluene-TPSR match well with the catalytic performances of MOF-Mn1Co1, MOF-Mn1Co2, and MOF-Mn2Co1, and in situ FITR proves that the benzoate route exists over MOF-Mn1Co1. It is found that a moderate ratio of Mn/Co (1:1) favors good low-temperature reducibility and high O/O, resulting in superior oxidation performance. However, the stability in the existence of water for MOF-Mn1Co1 is not satisfied, which should be overcome in the future.

摘要

锰钴混合金属氧化物被认为是挥发性有机化合物完全氧化的高效催化剂。在本研究中,采用纳米立方状金属有机框架(Mn[Co(CN)]·nH₂O)作为前驱体来制备具有不同锰钴摩尔比的锰钴氧化物,这对相结构和织构性质影响较小。所获得的具有均匀金属分散性的MOF-Mn₁Co₁富含高价态的表面锰和钴物种,导致甲苯完全氧化具有较高的低温催化活性。甲苯程序升温脱附(TPD)随后进行程序升温氧化(TPO)以及甲苯程序升温表面反应(TPSR)的结果与MOF-Mn₁Co₁、MOF-Mn₁Co₂和MOF-Mn₂Co₁的催化性能良好匹配,原位傅里叶变换红外光谱(FITR)证明在MOF-Mn₁Co₁上存在苯甲酸根途径。发现适度的锰钴比(1:1)有利于良好的低温还原性和高氧/氧比,从而产生优异的氧化性能。然而,MOF-Mn₁Co₁在有水存在时的稳定性不令人满意,这是未来需要克服的问题。

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